Femtosecond Laser Pulses Research Articles

The Impact of 1030 nm fs-Pulsed Laser on Enhanced Rayleigh Scattering in Optical Fibers.

This article presents a comprehensive study on the impact of irradiation optical fiber cores with a femtosecond-pulsed laser, operating at a wavelength of 1030 nm, on the signal amplitude in Rayleigh scattering-based optical frequency domain reflectometry (OFDR). The experimental study involves two fibers with significantly different levels of germanium doping: the standard single-mode fiber (SMF-28) and the ultra-high numerical aperture fiber (UHNA7). The research findings reveal distinct characteristics of reflected and scattered light amplitudes as a function of pulse energy. Although different amplitude changes are observed for the examined fibers, both can yield an enhancement of amplitude. The paper further investigates the effect of fiber Bragg grating inscription on the overall amplitude of reflected light. The insights gained from this study could be beneficial for controlling the enhancement of light scattering amplitude in fibers with low or high levels of germanium doping.

Optical and thermoplasmonic properties of core (AuxAg1- x)- shell (Au) nanostructures

The optical and thermoplasmonic properties of bimetallic nanoparticles (NPs) offer a wide range of possibilities for designing functional materials and innovative nanotechnological devices. Their exploration is generating increasing interest in experimental and theoretical scientific research. The combination of noble metals such as gold (Au) and silver (Ag) within the same nanostructure, in the form of an alloy or core/shell arrangement, presents several advantages and potential applications. In this paper, the finite element method (FEM) is used to study the optical response and nanoscale heat generation capability of bimetallic core/shell nanospheres composed of a mixed alloy (AuxAg1−x)-core and an Au-shell. First, we studied the surface plasmon resonance (SPR) properties by generating absorption spectra. Our results show that the position and amplitude of the SPR peak of these nanospheres are strongly influenced by the fractions of Au and Ag metals composing the core, as well as by the Au-shell thickness. In particular, the SPR-peak position can be adjusted between 535nm and 1085nm depending on the composition and structure of these NPs. Secondly, we studied the ability of these NPs to convert absorbed light into heat when exposed to either a continuous wave (cw) laser or a femtosecond pulsed (fs-pulsed) laser. The results demonstrate the ability to control the temperature generated by these NPs based on the core composition, Au-shell thickness, illumination intensity, and the type of illumination (cw or fs-pulsed). In particular, under fs-pulsed illumination, the internal temperature of the NPs is significantly higher than under cw illumination. These findings are crucial for the use of these alloy-core and Au-shell nanoparticles in various thermoplasmonic applications.

Research on picosecond synchronization control between synchrotron radiation X-ray pulse and femtosecond laser pulse on SSRF

The laser-pumped X-ray detection method is a crucial tool for investigating molecular dynamics, allowing researchers to study ultrafast structural changes within materials. This method demands extremely high precision in the synchronization and delay timing between the pump pulse and the probe pulse. In this study, we explored picosecond (ps)-level clock synchronization control between synchrotron radiation X-ray pulses and femtosecond (fs) laser pulses at the BL05U (d-Line) of the Shanghai Synchrotron Radiation Facility (SSRF). Utilizing the X-ray pulses generated by the 40 ps/0.3 mA electron beam bunch from the SSRF and femtosecond laser pulses with high repetition rates and high emission power, we conducted synchronization experiments. A custom-developed picosecond time synchronization control system and a high dynamic range X-ray streak camera with picosecond time resolution were used as detectors, enabling ultra-precise time synchronization monitoring of X-ray and laser pulses. This setup achieves higher time resolution without the need for photodiodes and oscilloscopes. Using the X-ray pulses as a stationary reference frame, we adjusted the clock synchronization control system to delay the laser pulses and measured their relative timing changes with the X-ray streak camera. The experiments demonstrated a time resolution better than 10 ps, providing a foundation for achieving 60 ps time resolution in laser-pumped X-ray detection experiments at the SSRF.

Power dependent tunable optical nonlinearity in Iron oxide/Borophene core-shell nanoparticles under ultrashort laser excitation

Two-dimensional (2D) nanomaterials find immense applications in ultrafast photonics and optical switching systems due to their fascinating nonlinear optical (NLO) characteristics. This work presents a systematic investigation of laser power-dependent nonlinear optical characteristics of borophene nanosheets in a core-shell nanostructure. For this purpose, we have synthesized Borophene encapsulated Iron oxide (Fe3O4) core-shell nanoparticles (Fe3O4/Borophene CSNPs). The CSNPs were synthesized by mixing and annealing sodium borohydride (NaBH4) as a boron precursor with iron oxide nanoparticles (Fe3O4 NPs) in a controlled environment using chemical vapor deposition technique (CVD) followed by characterization using XRD, FTIR Spectroscopy, UV–vis absorption spectroscopy, TEM, SEM, and EDX techniques. Magnetic properties were analyzed by a vibrating sample magnetometer (VSM) which shows that the saturation magnetization of Fe3O4 NPs increases after being encapsulated in borophene nanosheets. The role of borophene in modifying the NLO characteristics of Fe3O4/Borophene CSNPs was studied using a power-dependent Z-scan technique utilizing ultrashort (femtosecond) laser pulses at a wavelength of 800 nm in both open and close aperture configuration. It was found that borophene-coated Fe3O4 NPs reveal tunable NLO properties that resemble the NLO characteristics of borophene nanosheets with enhanced features. This provides insights into an interaction between materials in NLO phenomena and illustrates the distinctive performance of the core-shell nanostructure. The tunable NLO properties of Fe3O4/Borophene CSNPs offer an innovative approach for developing optoelectronics and ultrafast nonlinear photonic devices.

Optical characteristics and wavefront control of femtosecond laser pulses and their effect on the performance of diamond graphite electrodes

High purity diamond is an excellent material for making radiation hard detectors suitable for high-energy particle detection, cancer treatment and other fields. Electrodes are formed by the localized graphitization of the diamond bulk, where fine control of the manufacturing process is essential to the performance of the detector. The resistivity of the electrode formed by diamond graphitization significantly affects the performance of the detector. Femtosecond laser pulses interact with the material for a very short time (10-13 s), exhibiting a cold processing. In this paper, we utilize Spatial Light Modulators (SLM) to optimize the optical characteristics of the 800 nm femtosecond laser pulse and control the graphitization process. Our research focuses on the analysis of the influence exerted by the pulse characteristics on the diameter and resistivity of inscribed graphite structures. By examining these parameters, the study aims to refine the graphitization process, thereby optimizing the functional characteristics of the diamond-based detectors.

Mediating coherent acoustic phonon oscillation of a 2D semiconductor/3D dielectric heterostructure by interfacial engineering

Abstract Coherent acoustic phonon (CAP) oscillation of 2D layered semiconductor/3D dielectric heterostructure generated by femtosecond laser pulse excitation can realize ultrafast photoacoustic conversion, while the photoacoustic conversion efficiency suffers from interfacial phonon scatterings of simultaneously laser-induced lattice heat. Here, taking advantage of graphene’s high thermal conductivity and large acoustic impedance, we demonstrate that phonon scatterings can be markedly mediated in a MoS$_2$/graphene/glass heterostructure via femtosecond laser pump-probe measurements. Equilibrium temperatures of MoS$_2$ lattice have been cooled down by about 45 %. As a benefit, both lifetime of CAP oscillations and pump pulse-picosecond acoustic pulse energy conversion efficiency have been enhanced by a factor of about 2. Our results constitute insights into CAP manipulations via interfacial engineering, that are fundamentally important for ultrafast photoacoustics based on 2D layered semiconductors.

Optimized terahertz generation in BNA organic crystals with chirped Ti:sapphire laser pulses.

We report on the efficient generation of intense terahertz radiation from the organic crystal N-benzyl-2-methyl-4-nitroaniline pumped by chirped Ti:sapphire femtosecond laser pulses. The THz energy and spectrum as a function of the pump fluence and duration of the chirped laser pulses are studied systematically. For the appropriate positively chirped pump pulses, a significant boost in the THz generation efficiency by a factor of around 2.5 is achieved, and the enhancement of high-frequency components (>1 THz) shortens the THz pulse duration. Via complete characterization of THz properties and transmitted laser spectra, this nonlinear behavior is attributed to the extended effective interaction length for phase matching as a result of the self-phase modulation of the intense pump laser pulses. Numerical calculations well reproduce the experimental observation. Our results demonstrate a robust, efficient, strong-field (up to several MV/cm) THz source using the common sub-10 mJ and sub-100 fs Ti:sapphire laser systems without optical parametric amplifiers.

Amplification characteristics of N<i/>2+ lasing at multiple wavelengths generated by polarization-modulated femtosecond laser fields

Multiple gain routes complicate the amplification behaviors of N2+ lasing. A direct comparison of the amplification processes of various lasing lines of N2+ is still lacking to date, mainly because the efficient generation of different lasing lines requires different experimental conditions. In this work, to overcome the limitation, we use an intense polarization-modulated femtosecond laser pulse to simultaneously produce high-intensity N2+ lasing signals at 391 nm and 428 nm, permitting us readily performing their time-domain characterizations. Our results show that the primary amplification of 428-nm lasing is always retarded by a few picoseconds with respect to the probe pulse while the amplification of 391-nm lasing can be basically completed within the probe pulse duration at a relatively high gas pressure, and besides, the time duration of the former sustains several times longer than that of the latter. These observations indicate the non-negligible contribution of the initial electronic coherence established by the pump laser, apart from the external triggering pulse. For the 391-nm lasing, the seed amplification and superradiance can fiercely interplay within the probe pulse duration. However, for the 428-nm lasing, its amplification is in essence Raman-assisted superfluorescence due to the lacking of the initial electronic coherence and a direct triggering pulse. Our findings not only shed light on the physics of N2+ lasing but also promote the relevant studies on the collective emissions in the cascaded multi-level molecular ion system.

Hybrid Photoexcitation in Undoped Diamond by Mid-Infrared Femtosecond Laser Pulses

Direct interband and intragap photoexcitation by intense mid-infrared (4.0 and 4.7 μm) femtosecond (fs) laser pulses was explored in ultrapure chemical-vapor deposited (CVD) diamond via acquisition of characteristic ultraviolet photoluminescence of free excitons and A-band photoluminescence of electrons anchored at deep donor–acceptor or dislocation-related traps, respectively. At lower laser intensities (<10 TW/cm2) the excitonic photoluminescence yields exhibit highly nonlinear dependences with Iλ2-scaling and power slopes N ≈ 17 (4.0 μm) and 14 (4.7 μm), still insufficient to cross over the direct bandgap (≥6.5 eV) by ≈1.2 and 2.8 eV, respectively. Similarly high slope of ≈9 (4.7 μm) for intragap (≥3.5 eV) photo-population of donor–acceptor traps is still insufficient for their direct excitation by ≈1 eV. At the intermediate Iλ2-dependent values of the Keldysh parameter γ ∼ 1 such incomplete multiphoton excitation anticipates the hybrid total “multiphoton + tunneling” photoexcitation generally predicted by the Keldysh theory, but never unambiguously experimentally demonstrated. At higher laser intensities (>10 TW/cm2) both the excitonic and A-band photoluminescence yields exhibit (sub)linear slopes, apparently, indicating formation of more strongly absorbing electron–hole plasma. These findings shed light on the hybrid multiphoton + tunneling character of Keldysh photoexcitation at intermediate values γ and pave the way to defect/impurity band engineering of intragap nonlinear optical properties in bulk dielectrics for their precise fs-laser nanomodification.

Doping engineering of NiO–Zn nanofilms for modulation of morphological structure and ultrafast nonlinear optical response at 515 nm

In this work, to investigate the metal doping on the third-order nonlinear optical properties of NiO thin films under femtosecond pulsed laser excitation, pure NiO and 2w,4w,6w,8w Zn doped-NiO nanofilms were prepared by DC-RF co-sputtering technique. Then, the nonlinear absorption properties and nonlinear refractive properties of the five samples were investigated using the femtosecond laser at a wavelength of 515 nm. The experimental results show that the nonlinear absorption and nonlinear refractive properties of NiO are enhanced by the doped metal as well as the effect of defects. In addition, by varying the pump light intensity, we observed the transition of nonlinear absorption from the coexistence of saturated absorption and reverse saturated absorption to reverse saturated absorption. We established a multi-energy level system to interpret the nonlinear absorption and nonlinear refractive results, which broadens the application of NiO thin films in the field of nonlinear optics.

Optically Tunable Many-Body Exciton-Phonon Quantum Interference.

This study introduces a novel paradigm for achieving widely tunable many-body Fano quantum interference in low-dimensional semiconducting nanostructures, beyond the conventional requirement of closely matched energy levels between discrete and continuum states observed in atomic Fano systems. Leveraging Floquet engineering, the remarkable tunability of Fano lineshapes is demonstrated, even when the original discrete and continuum states are separated by over 1eV. Specifically, by controlling the quantum pathways of discrete phonon Raman scattering using femtosecond laser pulses, the Raman intermediate states across the excitonic Floquet band are tuned. This manipulation yields continuous transitions of Fano lineshapes from antiresonance to dispersive and to symmetric Lorentzian profiles, accompanied by significant variations in Fano parameter q and Raman intensity spanning 2 orders of magnitude. A subtle shift in the excitonic Floquet resonance is further shown, achieved by controlling the intensity of the femtosecond laser, which profoundly modifies quantum interference strength from destructive to constructive interference. The study reveals the crucial roles of Floquet engineering in coherent light-matter interactions and opens up new avenues for coherent control of Fano quantum interference over a broad energy spectrum in low-dimensional semiconducting nanostructures.

Pressure scaling of femtosecond laser filamentation in air: Prospects for long-range atmospheric propagation

The principal trend of the last decades is the use of laser systems generating ultrashort (femtosecond) laser pulses of gigawatt and terawatt power in various spheres of human activity, in particular, in atmospheric researches. One of the important challenges within this problem is the use of the unique nonlinear optical phenomena manifesting in the atmosphere as pulse self-focusing, light-induced ionization of the medium, plasma generation and laser filamentation for remote laser diagnostics of the aerosol-gas constituents and efficient delivery of concentrated optical energy over long distances in the atmosphere. This brings to the forefront the problem of increasing the actual length of the nonlinear interaction of an ultrashort laser pulse with medium to kilometer distances whereas real physical length of most existing optical paths is usually limited by several hundred meters. We propose and theoretically substantiate an effective way to solve the problem of long-range atmospheric filamentation by transforming the propagation medium itself using short laboratory traces and optical cuvettes with gases of increased (over-atmospheric) pressure. Following the scaling laws of the optical characteristics of pressurized medium, the coefficients describing the interaction between optical wave and medium increase along with the increase in gas pressure. By the numerical simulations in the framework of the nonlinear Schrodinger equation, we show that this makes it possible to emulate kilometers-long atmospheric traces for laser beams of centimeter diameter and terawatt pulse power on the laboratory scale (tens of meters).

Using femtosecond laser pulses to investigate the thickness-dependent nonlinear optical properties of nickel oxide thin films and their potential use as optical limiters

In this study, the Z-scan technique was used to investigate the nonlinear optical properties of nickel oxide (NiO) thin films of various thicknesses. Direct current (DC) sputtering was used to deposit single-phase NiO thin films with thicknesses of 280, 350, and 470 nm onto a soda-lime glass substrate. The film structure was measured using X-ray diffraction (XRD) and scanning electron microscopy (SEM), while the linear optical properties were measured using a UV-Vis spectrophotometer. NiO thin films were irradiated with 100 fs laser pulses at various excitation wavelengths and excitation powers to determine the nonlinear absorption coefficient and nonlinear refractive index. The NiO films were found to have reverse saturable absorption and self-focusing behavior. As the thickness of the NiO film increases, both the nonlinear absorption coefficient and nonlinear refractive index decrease. Additionally, the investigation of the optical limitations of NiO thin films revealed a definite association with the thickness of the NiO thin film.

Infrared microlens formation on chalcogenide polymer surface via femtosecond laser pulse ablation

In this study, we introduced micro-optical surface formation via femtosecond (fs) laser pulse scanning to chalcogenide polymer (ChP), a promising material for cost-effective infrared applications. Employing this method, we successfully fabricated a large-area poly(sulfur-random-(1,3-diisopropenylbenzene)) (S-r-DIB) microlens array (MLA) component. Each micro-concave spherical surface was crafted with a single fs laser pulse, serving as a micro-concave lens surface. We achieved a quasi-periodic MLA sample with over 2 × 105 micro-lenslets within a 10 mm × 10 mm footprint. Additionally, precise locating of laser pulse irradiation enabled us to create a hexagonal MLA with a filling factor over 37 %. Morphological investigations and imaging tests confirmed the adequate surface quality of the fabricated components, with its uniformity revealed by the virtual foci grid in near infrared region. To elucidate the forming conditions and mechanisms, we studied the evolution of surface morphology under various laser irradiation conditions. Laser induced damage thresholds of S70-r-DIB30 were experimentally determined for both 800 nm and 400 nm wavelengths under single- and multi-pulse irradiation scenarios. We identified the optimal fabrication fluence window as 115–205 mJ/cm2 with 800 nm single-pulse irradiation. The bandgap of the S70-r-DIB30 was estimated as 2.06 eV, and energy band analysis confirmed distinctions in ablation morphology. Furthermore, we investigated sub-surface morphology evolution using orthogonal ultrafast pump–probe imaging, revealing diversity compared to traditional inorganic and polymeric optical materials due to differing absorption and etching mechanisms. The elastic wave velocity of 3.2 km/s in this ChP and etching velocity of 0.7 μm/pulse were experimentally determined. These findings deepen our understanding of ChP material interaction with fs lasers, offering insights for potential applications such as surface engineering, substrate cutting, and micro-structure formation.

Relief of pain in mice by an antibody with high affinity for cell adhesion molecule 1 on nerves

AimsCell adhesion molecule 1 (CADM1) is a member of the immunoglobulin superfamily and is abundantly expressed on nerve fibers. Recently, the anti-CADM1 ectodomain antibody 3E1 has proven useful as a drug delivery vector for CADM1-expressing cells in vitro. When injected subcutaneously into mice, whether 3E1 accumulates on nerve fibers and serves as an analgesic was examined. Main methodsInjected 3E1 was detected by immunohistochemistry and double immunofluorescence. Analgesic effects were verified by a formalin-induced chemical-inflammatory pain test and video-recorded behavior analysis that were performed 6, 12, and 24 h after antibody injection. Primary cultures of mouse dorsal root ganglion (DRG) cells were incubated with 3E1 and expressions of CADM1 and its key downstream molecules were examined by Western blot analyses and live cell imaging. DRG cells were loaded with a Ca2+ fluorescent indicator Fluo-8 and a femtosecond laser pulse was irradiated near the cell body to mechanically stimulate the nerves. Key findingsSubcutaneously injected 3E1 was widely localized almost exclusively on peripheral nerve fibers in the dermis. In formalin tests, 3E1-injected mice exhibited less pain-related behavior than control mice. When 3E1 was added to DRG cell cultures, it localized to neurites and resulted in decreased expression of CADM1, increased phosphorylation of Src and Akt, and CADM1-3E1 complex formation. Femtosecond laser-induced stimulation transmission along neurites was clearly visualized by Fluo-8 fluorescence in control cells, whereas it was markedly suppressed in 3E1-treated cells. Significance3E1 was suggested to be a potential long-acting analgesic based on its high affinity for CADM1.

Direct Writing of SERS Substrates Using Femtosecond Laser Pulses.

Achieving a high-density, repeatable, and uniform distribution of "hotspots" across the entire surface-enhanced Raman scattering (SERS) substrate is a current challenge in facilitating the efficient preparation of large-area SERS substrates. In this study, we aim to produce homogeneous surface-enhanced Raman scattering (SERS) substrates based on the strong interaction between femtosecond laser pulses and a thin film of colloidal gold nanoparticles (AuNPs). The SERS substrate we obtained consists of irregularly shaped and sharp-edged gold nanoparticle aggregates with specially extruding features; meanwhile, a large number of three-dimensional AuNP stacks are produced. The advantages of such configurations lie in the production of a high density of hotspots, which can significantly improve the SERS performance. When the laser fluence is 5.6 mJ/cm2, the substrate exhibits the best SERS enhancement effect, and a strong SERS signal can still be observed when testing the concentration of R6G at 10-8 mol/L. The enhancement factor of such SERS substrates prepared using femtosecond laser direct writing is increased by 3 orders of magnitude compared to the conventional furnace annealing process. Furthermore, the relative standard deviation for the intensities of the SERS signals was measured to be 5.1% over an area of 50 × 50 μm2, indicating a highly homogeneous SERS performance and excellent potential for practical applications.

Repetition‐Rate and Wavelength Flexible Femtosecond Laser Pulse Generation

AbstractCompared to mode‐locked oscillators, gain‐switched diodes (GSD) have the key advantage of repetition‐rate agility. Yet, large pulse duration and poor coherence of the GSD pulses greatly limit their applications. Here, a GSD‐pumped Raman fiber amplifier is demonstrated, which can effectively generate femtosecond laser pulses with both repetition‐rate and wavelength agility. It is proved that both nonlinear optical gain and single‐frequency seed in the fiber amplifier play critical roles for improving the coherence of the generated laser pulses. In the experimental demonstration, pumped by 1065 nm GSD pulses, the nonlinear fiber amplifier can generate highly coherent 1121 nm femtosecond Raman pulses with up to 80.2% conversion efficiency. The Raman pulses can maintain high performance within the repetition‐rate tuning range from 1 to 150 MHz. The potential for generating 1178 nm femtosecond Raman pulses is also demonstrated with an optical conversion efficiency of 63.8%. This all‐fiber based femtosecond laser with both repetition‐rate and wavelength agility is a promising light source for applications such as nonlinear microscopy and micromachining.

Ultrafast optical pumping induced polarity and chirality reversal of Néel skyrmions in amorphous GdFeCo ferrimagnet

The development of next-generation data storage devices relies on the efficient control of topological spin textures at ultrafast timescales with minimal energy consumption. Here, we theoretically investigate the switching of the magnetic skyrmion in ferrimagnetic GdFeCo utilizing the helicity-independent all-optical switching (HI-AOS) driven by femtosecond laser pulses. Our study demonstrates the switching of Néel skyrmion between the two degenerate skyrmion ground states having opposite polarity and chirality. A systematic study was done by varying the laser fluence, and we found that single-shot skyrmion switching is observed for a range of fluence values, where optically induced magnetization switching is observed. The present study proves that HI-AOS is a potential mechanism for switching magnetic skyrmion at ultrafast timescales. Our results offer significant insight into implementing optical writing skyrmion-based memory devices.

Determination of product ions emerged from dications by varying retarding electric field in reflectron time-of-flight mass spectrometer supported by ion trajectory simulations

Investigation of the metastable dissociations clarifies the characteristics of ionic states. Tandem mass spectrometry using an ion trap mass spectrometer, a time-of-flight mass spectrometer (TOF-MS), and the combination of those spectrometers were used for the analysis of metastable dissociation. However, investigation of the metastable dissociations of multiply charged ions is not straightforward because collision-induced charge transfer reactions to lose charges should be avoided. TOF-MS equipped with a reflectron (refTOF-MS) maintained under high vacuum condition is one of the suitable instruments. However, another difficulty arises due to the working principle of refTOF-MS: The product ions whose m/z is greater than that of multiply charged precursor ions can pass through a reflectron under the experimental conditions for detecting the product ions of a singly charged precursor ion. In this study, we report the ionization of decafluorobiphenyl (DFB) by femtosecond laser pulses and the determination of the product ions emerged from doubly charged precursor ions using a refTOF-MS. Detection of ions behind a reflectron by varying the retarding potential of a reflectron enables us to identify the m/z of product ions in two ways: measurement of the threshold retarding potential reflecting product ion; comparing the relative flight time of the product ions obtained by experiments and ion trajectory simulations. We have reported three and one metastable dissociation channels of DFB+ and DFB2+, respectively, by a conventional product ion analysis, that is the selection of a precursor ion and its product ions using an ion gate followed by the reflection and separation of them by a reflectron. In this study, we further identified the products that passed through a reflectron: charge transfer product of C2+; the product ion of C4F22+ which is a secondary product of DFB ion; the product ion of DFB2+. The detection of the product ions that passed through a reflectron expanded the measurable m/z range of product ions emerged from doubly charged precursor ions.

Considerations for ultrafast photomagnetism in manganese(III)-based single-molecule magnets

Manipulation of magnetic materials is a cornerstone of digital data storage technologies. Recently, it has been shown that femtosecond laser pulses are capable of switching the magnetization in a material between two stable configurations faster than ever before. One state-of-the-art method is to use laser pulses to control the magnetic anisotropy by photoexciting crystal-field transitions. The photoinduced change in anisotropy applies a torque to the magnetic moment, which reorientates it in a different direction. So far, research has focused solely on condensed matter materials. However, there is a huge variety of molecule-based magnetic materials that have been and continue to be developed. In particular, single-molecule magnets (SMMs) provide a highly tunable platform and have the added advantage of operating on nanometer length scales. This review discusses recent research in the area of ultrafast magnetism in SMMs, with a focus on manganese(III)-based transition metal complexes. Experimental data are reviewed, showing that control of the strength of the photoinduced anisotropy, the lifetime of excited states, and the dephasing times are possible and can be used to develop some design criteria for the best optically controllable SMMs.